Conceptual design of tetraazaporphyrin- and subtetraazaporphyrin-based functional nanocarbon materials: electronic structures, topologies, optical properties, and methane storage capacities

A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silico design. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The...

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Published inPhysical chemistry chemical physics : PCCP Vol. 18; no. 19; pp. 13503 - 13518
Main Authors Belosludov, Rodion V, Rhoda, Hannah M, Zhdanov, Ravil K, Belosludov, Vladimir R, Kawazoe, Yoshiyuki, Nemykin, Victor N
Format Journal Article
LanguageEnglish
Published England 2016
Subjects
Bridging
Carbon
Electronic structure
Mathematical analysis
Methane
Nanostructure
Optical properties
Topology
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Abstract A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silico design. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The stability of nanocages of Oh symmetry and nanobarrels of D4h symmetry was revealed on the basis of DFT and MD calculations, whereas their optical properties were assessed using a TDDFT approach and a long-range corrected LC-wPBE exchange-correlation functional. It was shown that the electronic structures and vertical excitation energies of the functional nanocage and nanobarrel structures could be easily tuned via their size, topology, and the presence of bridging sp(3) carbon atoms. TDDFT calculations suggest significantly lower excitation energies in fully conjugated nanocages and nanobarrels compared with systems with bridging sp(3) carbon fragments. Based on DFT and TDDFT calculations, the optical properties of the new materials can rival those of known quantum dots and are superior to those of monomeric phthalocyanines and their analogues. The methane gas adsorption properties of the new nanostructures and nanotubes generated by conversion from nanobarrels were studied using an MD simulation approach. The ability to store large quantities of methane (106-216 cm(3) (STP) cm(-3)) was observed in all cases with several compounds being close to or exceeding the DOE target of 180 cm(3) (STP) cm(-3) for material-based methane storage at a pressure of 3.5 MPa and room temperature.
AbstractList A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silico design. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The stability of nanocages of O h symmetry and nanobarrels of D 4h symmetry was revealed on the basis of DFT and MD calculations, whereas their optical properties were assessed using a TDDFT approach and a long-range corrected LC-wPBE exchange–correlation functional. It was shown that the electronic structures and vertical excitation energies of the functional nanocage and nanobarrel structures could be easily tuned via their size, topology, and the presence of bridging sp 3 carbon atoms. TDDFT calculations suggest significantly lower excitation energies in fully conjugated nanocages and nanobarrels compared with systems with bridging sp 3 carbon fragments. Based on DFT and TDDFT calculations, the optical properties of the new materials can rival those of known quantum dots and are superior to those of monomeric phthalocyanines and their analogues. The methane gas adsorption properties of the new nanostructures and nanotubes generated by conversion from nanobarrels were studied using an MD simulation approach. The ability to store large quantities of methane (106–216 cm 3 (STP) cm −3 ) was observed in all cases with several compounds being close to or exceeding the DOE target of 180 cm 3 (STP) cm −3 for material-based methane storage at a pressure of 3.5 MPa and room temperature.
A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silico design. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The stability of nanocages of Oh symmetry and nanobarrels of D4h symmetry was revealed on the basis of DFT and MD calculations, whereas their optical properties were assessed using a TDDFT approach and a long-range corrected LC-wPBE exchange-correlation functional. It was shown that the electronic structures and vertical excitation energies of the functional nanocage and nanobarrel structures could be easily tuned via their size, topology, and the presence of bridging sp(3) carbon atoms. TDDFT calculations suggest significantly lower excitation energies in fully conjugated nanocages and nanobarrels compared with systems with bridging sp(3) carbon fragments. Based on DFT and TDDFT calculations, the optical properties of the new materials can rival those of known quantum dots and are superior to those of monomeric phthalocyanines and their analogues. The methane gas adsorption properties of the new nanostructures and nanotubes generated by conversion from nanobarrels were studied using an MD simulation approach. The ability to store large quantities of methane (106-216 cm(3) (STP) cm(-3)) was observed in all cases with several compounds being close to or exceeding the DOE target of 180 cm(3) (STP) cm(-3) for material-based methane storage at a pressure of 3.5 MPa and room temperature.
A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silicodesign. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The stability of nanocages of O sub(h) symmetry and nanobarrels of D sub(4h) symmetry was revealed on the basis of DFT and MD calculations, whereas their optical properties were assessed using a TDDFT approach and a long-range corrected LC-wPBE exchange-correlation functional. It was shown that the electronic structures and vertical excitation energies of the functional nanocage and nanobarrel structures could be easily tuned via their size, topology, and the presence of bridging sp super(3) carbon atoms. TDDFT calculations suggest significantly lower excitation energies in fully conjugated nanocages and nanobarrels compared with systems with bridging sp super(3) carbon fragments. Based on DFT and TDDFT calculations, the optical properties of the new materials can rival those of known quantum dots and are superior to those of monomeric phthalocyanines and their analogues. The methane gas adsorption properties of the new nanostructures and nanotubes generated by conversion from nanobarrels were studied using an MD simulation approach. The ability to store large quantities of methane (106-216 cm super(3) (STP) cm super(-3)) was observed in all cases with several compounds being close to or exceeding the DOE target of 180 cm super(3) (STP) cm super(-3) for material-based methane storage at a pressure of 3.5 MPa and room temperature.
Author Belosludov, Rodion V
Rhoda, Hannah M
Belosludov, Vladimir R
Zhdanov, Ravil K
Nemykin, Victor N
Kawazoe, Yoshiyuki
Author_xml – sequence: 1
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  organization: Institute for Materials Research, Tohoku University, Sendai, 980-85577, Japan. rodion@imr.tohoku.ac.jp
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  givenname: Hannah M
  surname: Rhoda
  fullname: Rhoda, Hannah M
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  surname: Zhdanov
  fullname: Zhdanov, Ravil K
  organization: Nikolaev Institute of Inorganic Chemistry, SB RAS, Lavrentiev 3, Novosibirsk 630090, Russia
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  givenname: Vladimir R
  surname: Belosludov
  fullname: Belosludov, Vladimir R
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  givenname: Yoshiyuki
  surname: Kawazoe
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  organization: New Industry Creation Hatchery Center, Tohoku University, 6-6-4 Aoba, Aramaki, Sendai 980-8579, Japan
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  givenname: Victor N
  surname: Nemykin
  fullname: Nemykin, Victor N
  email: vnemykin@d.umn.edu
  organization: Department of Chemistry and Biochemistry, University of Minnesota Duluth, Duluth, Minnesota 55812, USA. vnemykin@d.umn.edu
BackLink https://www.ncbi.nlm.nih.gov/pubmed/27128697$$D View this record in MEDLINE/PubMed
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Snippet A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been...
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SubjectTerms Bridging
Carbon
Electronic structure
Mathematical analysis
Methane
Nanostructure
Optical properties
Topology
Title Conceptual design of tetraazaporphyrin- and subtetraazaporphyrin-based functional nanocarbon materials: electronic structures, topologies, optical properties, and methane storage capacities
URI https://www.ncbi.nlm.nih.gov/pubmed/27128697
https://search.proquest.com/docview/1815995183
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